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The discovery of two-dimensional systems hosting intrinsic magnetic order represents a seminal addition to the rich landscape of van der Waals materials. CrI₃is an archetypal example, where the interdependence of structure and magnetism, along with strong light-matter interactions, provides a new platform to explore the optical control of magnetic and vibrational degrees of freedom at the nanoscale. However, the nature of magneto-structural coupling on its intrinsic ultrafast timescale remains a crucial open question. Here, we probe magnetic and vibrational dynamics in bulk CrI₃using ultrafast optical spectroscopy, revealing spin-flip scattering-driven demagnetization and strong transient exchange-mediated interactions between lattice vibrations and spin oscillations. The latter yields a coherent spin-coupled phonon mode that is highly sensitive to the driving pulse’s helicity in the magnetically ordered phase. Our results elucidate the nature of ultrafast spin-lattice coupling in CrI₃and highlight its potential for applications requiring high-speed control of magnetism at the nanoscale.

 

Developing functional, cleavable two-dimensional materials for use in next generation devices has recently become a topic of considerable interest due to their unique properties. Of particular interest, transition metal halides CrI3 and CrCl3 have shown to be good contenders for tunable and cleavable magnetic materials due to their unique magnetic properties in the monolayer. 

van der Waals (vdW) magnetic materials show promise in being the foundation for future spintronic technology. The magnetic behavior of Fe2.7GeTe2 (FGT), a vdW itinerant ferromagnet, was investigated before and after proton irradiation. Proton irradiation of the sample was carried out at a fluence of 1×1018 cm-2. The magnetization measurements revealed a small increase of saturation magnetization (Ms) of about 4% upon proton irradiation of the sample, in which, the magnetic field was applied parallel to the c-axis. X-ray photoelectron spectroscopy for pristine and irradiated FGT revealed a general decrease in intensity after irradiation for Ge and Te and an increase in peak intensity of unavoidable surface iron oxide. Furthermore, no noticeable change in the Curie temperature (TC =152 K) is observed in temperature dependent magnetization variation. This work signifies the importance of employing protons in tuning the magnetic properties of vdW materials. 

The bulk van der Waals crystal Mn3Si2Te6 (MST) has been irradiated with a proton beam of 2 MeV at a fluence of 1×1018 H+ cm-2. The temperature dependent magnetization measurements show a drastic decrease in the magnetization of 49.2% in the H//c direction observed in ferrimagnetic state. This decrease in magnetization is also reflected in the isothermal magnetization curves. No significant change in the ferrimagnetic transition temperature (75 K) was reflected after irradiation. Electron paramagnetic resonance (EPR) spectroscopy shows no magnetically active defects present after irradiation. Here, experimental findings gathered from MST bulk crystals via magnetic measurements, magnetocaloric effect, and heat capacity are discussed.